CN106219600A - A kind of method utilizing two-dimensional material suppression perovskite auger recombination - Google Patents
A kind of method utilizing two-dimensional material suppression perovskite auger recombination Download PDFInfo
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Abstract
The invention belongs to photoelectric technology Material Field, be specifically related to a kind of method utilizing two-dimensional material suppression perovskite auger recombination, including: first it is chemically synthesized perovskite micron order club shaped structure；Then being shifted by wet method, shift Graphene on the glass substrate, add last layer two-dimensional material Graphene below perovskite, for the Raman spectrum of Graphene, the peak value at G peak and 2D peak is all higher than 0.8 × 10k a.u..For can the application in the delivery efficiency that field of semiconductor lasers reduces auger recombination, increase laser lay the foundation, for providing thinking in the application improving the photoelectric fields such as the efficiency of solaode, OLED.
Description
Technical field
The invention belongs to field of photoelectric technology, be specifically related to a kind of side utilizing two-dimensional material suppression perovskite auger recombination
Method.
Background technology
Research for lead halide perovskite the most still concentrates in its laser behavior.Perovskite nanometer rods Low threshold,
The performance of high q-factor to confirming widely.But to the performance of perovskite microlaser under high excitation energy
Study or relatively small number of.
In the case of high pumping density, use two-dimensional material, such as Graphene, prepare perovskite/Graphene system
System is relative to simple perovskite microlaser, and the output intensity of light adds 4 times, and threshold value reduces nearly 20%.Now calcium
Titanium ore microlaser also demonstrates a parallel even negative energy slope, and whole output energy is the most saturated.
Explain that the output energy increase of perovskite/Graphene system, threshold value reduce, main reasons is that Graphene this two
Dimension material as the carrier of electronics, has longer at electron diffusion length, and the electronics and the hole that are is separated to different
Region, effectively reduces the auger recombination of exciton.
Biennium lead halide perovskite microlaser in the past is studied the most widely, perovskite nanometer rods
The characteristic of Low threshold and high q-factor it turned out.But most research the most still concentrates on the sight to perovskite laser behavior
Examine.Under high excitation energy, the performance of perovskite microlaser is the most more studied, and these performances are in display
Critically important application is had on device and lasing light emitter.
It in contrast to traditional thin-film solar cells, the application on the solar cell of lead halide perovskite, can be reduced me
Preparation cost.Because we are perovskites prepared by the chemical synthesis by solution.The light conversion of this perovskite is
Number height, has high external quantum efficiency and high gain coefficient.Meanwhile, the halogen adulterated by change: Cl, Br, I, can
With the position of the fluorescence emission wavelengths of accurate regulation and control perovskite from ultraviolet to near-infrared.And the lead bromide calcium titanium that we are studied
The transmitting wavelength in ore deposit is in the position of about 550nm.
Certainly, in the past few years, a lot of team the most each confirm monocrystalline lead halide perovskite micron block, micron
Rod, the laser behavior of nanometer rods are, and the performance of Low threshold, high q-factor is also it has been reported that out.Meanwhile, double light of perovskite
The non-linear behaviour the most very in-depth study such as son absorption and two-photon pumping transmitting.Some application of perovskite, such as
Say that the freezing and adjustable perovskite microlaser of laser is recognized the most widely.But laser behavior for perovskite is outstanding
It is that the performance under high pumping intensity is seldom discussed by people and studies.How to go effectively to change threshold value and Q-value, in research
All it is particularly important in the performance of the perovskite under high pumping intensity and semiconductor device preparation.
Summary of the invention
The technical problem existed in view of prior art, under high pump energy, perovskite microlaser
The regulation and control of threshold value and Q-value seldom come into question and study, and the reason of this modulation is seldom by detailed explanation.The present invention provides
A kind of method utilizing two-dimensional material suppression perovskite auger recombination, specifically:
Described method includes: be first chemically synthesized perovskite micron order club shaped structure；Then shifted by wet method,
Shift Graphene in substrate of glass, add last layer two-dimensional material Graphene below perovskite, for the Raman spectrum of Graphene, G
The peak value at peak and 2D peak is all higher than 0.8 × 10k a.u..
We devise the system of perovskite/Graphene, as electron acceptor and have long current-carrying by Graphene
The character of carrier diffusion length, under high pump light intensities, effectively reduces the threshold value of perovskite microlaser, increases
The intensity of output light.And reduce the binding energy of exciton from Graphene first and decrease the auger recombination angle of exciton to threshold
The phenomenon of the intensity increase that value reduces and exports light is explained.
For the Raman spectrum of Graphene, the peak value at G peak is 8505a.u..Peak for the Raman spectrum 2D peak of Graphene
Value is 13845a.u..
Still a further object of the present invention is to provide the system of a kind of perovskite/Graphene, it is characterised in that and described perovskite/
The system of Graphene is prepared by described method, and system and the Perovskite Phase of described perovskite/Graphene compare, threshold value
Reduce nearly 20%.
Output light intensity under identical pump intensity increases nearly 4 times.The system of described perovskite/Graphene and calcium
Titanium ore compares, and exciton bind energy have dropped nearly 26%.
Under identical pump intensity, the halfwidth of perovskite fluorescence spectrum is than the fluorescence spectrum of perovskite/Graphene
The little nearly 1nm of halfwidth.
Still a further object of the present invention is to provide a kind of electricity original paper, containing the system of described perovskite/Graphene.
Described electricity refers to the photovoltaic industry such as solaode, OLED.Described electricity original paper include perovskite laser instrument,
Semiconductor laser etc..
The most detailed concrete being described as follows: in this design, we are synthesized by the method for chemosynthesis
CH3NH3PbBr3Perovskite, in order to get rid of the impact of mode competition and Mode Coupling, we have chosen the rod launching single-mode laser
Shape perovskite microlaser cavity, such microlaser cavity has good local effect to pump light, thus under high pump light density
There is high q-factor and obtain characteristic, stronger laser can be launched simultaneously.We pass through micromanipulative technique, will by optical fiber
CH3NH3PbBr3Perovskite micron bar transfers to be formed on the Graphene of few layer the system of perovskite/Graphene.It was found that it is defeated
The light intensity gone out increases more than 4 times when being on simple glass relative to perovskite and threshold value reduces nearly 20%.Explain it
Reason, it is believed that, owing to Graphene is as the receptor of electronics, efficiently separate exciton, by perovskite/Graphene system circle
Electronics and hole at face separate in different regions, thus reduce the auger recombination between exciton.Because auger recombination with
The separation of exciton is relevant with the transfer of electric charge, so in order to verify Auger process, we consider from the binding energy of exciton.We
Sample is put in liquid nitrogen cryogenics thermostat, measure perovskite and perovskite/Graphene system temperature respectively from 10K to room temperature
Fluorescence, is finally gone out the binding energy (Eb) of exciton, thus obtains the exciton confinement of simple perovskite by Arrhenius equation model
Can be 14.8meV, the exciton bind energy of perovskite/Graphene system be 10.9meV, and what this result will be apparent from presents graphite
The impact on perovskite exciton bind energy of the alkene layer.Meanwhile, auger recombination also can be embodied on the width of spectrum, when auger recombination is subject to
To suppression, the width of spectrum will increase.It is shown experimentally that, under identical pump intensity, the fluorescence of simple perovskite
A halfwidth nearly 1nm less than the halfwidth of the fluorescence spectrum of perovskite/Graphene of spectrum.
The method of the present invention can be widely used in photoelectric field, the such as photovoltaic industry such as solaode, OLED, tool
The application mode of body includes: perovskite laser instrument, semiconductor laser etc..
" auger recombination " of the present invention refers to the corresponding recombination process of Auger transition.
The present invention includes relative to the beneficial effect of prior art:
1) present invention prepares simply, and the technology of the perovskite of chemical synthesis synthesizing micron-grade and wet method transfer Graphene is equal
With comparative maturity, whole preparation process is simple and cost is relatively low, and has no that the material the two method obtained is combined use
Situation.
2) operation and the comparison of the method for the present invention are easy, and method is simple, feasible, has a extensive future.
3) effect that perovskite threshold value is reduced, increases its laser output energy by the two-dimensional material with Graphene as representative
Phenomenon is obvious, and by the interpretation of auger recombination, either theory is the most reliable.Finally demonstrate high pump
Under the light intensity of Pu, Graphene reduces the reasonability of perovskite/Graphene system auger recombination.For dropping in field of semiconductor lasers
Low auger recombination, the application increased in the delivery efficiency of laser lay the foundation, for improving the efficiency of solaode, OLED
Thinking is provided Deng the application of photoelectric field.
Accompanying drawing explanation
Fig. 1, the Scanning Electron microscope photograph of chemosynthesis perovskite；
Fig. 2, Graphene detection picture, (a) Graphene microscope photograph, (b) graphite Raman spectrogram；
Fig. 3, the spectrogram of perovskite and threshold curve schematic diagram, the laser spectrum of (3a) perovskite and threshold curve,
(3b) threshold curve of perovskite/Graphene；
Fig. 4, the binding energy schematic diagram of exciton, the exciton bind energy of (4a) perovskite, (4b) perovskite/Graphene system
Exciton bind energy；
Fig. 5, spectral width schematic diagram, the laser spectrum width of (5a) perovskite and perovskite/Graphene, (5b) is by swashing
The halfwidth that light spectrum simulation goes out.
Detailed description of the invention
Below in conjunction with embodiment and accompanying drawing, the present invention is described in further detail, but the embodiment of invention is not limited to
This.
Embodiment:
First we are by being chemically synthesized perovskite micron order club shaped structure, SEM picture such as Fig. 1 of result after synthesis
Shown in, certain chemosynthesis has the shortcoming of randomness, but in this visual field, due to the control of synthesis condition, major part is all
Our required club shaped structure, simultaneously from size for, be also substantially the same.Thus meet our later experiments
The essential condition that can repeat.
Such as: concrete attainable chemical parameters method is as follows
Weigh the methyl bromide ammonium (CH of certain mass respectively3NH3And lead bromide (PbBr Br)2) pressed powder, it is dissolved in respectively
Two parts prepare, in dimethylformamide (DNF) solution of ready respective volume in advance, to be prepared as two parts of concentration and be
Methyl bromide ammonium (the CH of 0.1mol/l3NH3Br) solution and lead bromide (PbBr2) solution.After two parts of solution hybrid reactions, join
It is set to the methyl bromide ammonium lead bromide (CH for concentration is 0.05mol/l3NH3Br·PbBr2) solution.Respectively use acetone and
Isopropanol ultrasonic cleaning has been cut into the sheet glass of suitable dimension, and sheet glass is positioned over the polytetrafluoroethyl-ne of one piece of suitable dimension
On alkene platform, platform is placed in dichloromethane (DCM) solution equipped with suitable volumes, and dichloromethane must not flood flat
Platform, liquid level should be placed in below platform, then be dripped on sheet glass by the solution configured.Microporous freshness-keeping film is finally used to seal
Beaker, by whole system as in the preferable fume hood of ventilated environment, carries out synthetically grown.
Shifted by wet method, shift Graphene on the glass substrate.And drawing of the Graphene surveyed by Raman spectrometer
Graceful spectrum judges the thickness of Graphene.The optical microscope picture of Graphene such as Fig. 2 a and Raman spectrogram are as shown in Figure 2 b.
It will be seen that we can shift large-area Graphene by the method that wet method shifts from figure.And for graphite
The Raman spectrum of alkene, when the peak value at G peak and 2D peak is less than or equal to 0.8, one can consider that Graphene is monolayer, and we
Result approximate 0.9, more than 0.8, one can consider that our Graphene is few layer.
Such as, concrete attainable wet method transfer parameters method is as follows:
(1) Graphene/Copper Foil being cut into target sizes, about 1x1cm size, idea is not touched during cutting
The upper surface of Copper Foil, it is to avoid Graphene is caused damage by mechanical damage；
(2) configuring the etching solution of copper, what we typically chose is all ferric chloride solution, and what we chose here is to make
Use FeCl3(6H2O)、HCl、H2O, according to certain proportioning, is the FeCl of 25%wt by stirring and dissolving compound concentration3Solution；
(3) sol evenning machine colloidal sol on the sample of Copper Foil/Graphene, spin coating A4PMMA are used.So that final glue holds
Easily being removed, we select rotating speed to be 4000 to rotate into row spin coating, and the thickness of final PMMA is about 270nm.PMMA/ by even good glue
Graphene/Copper Foil is as the cool 5-10min of air at room temperature；
(4) the PMMA/ Graphene/copper foil sample after above-mentioned colloidal sol is placed on the drying glue platform of 60 DEG C heating 3min, makes
PMMA is cured；
(5) by the most cooled sample gently be put into the FeCl prepared3In solution, wait the dissolving of copper, wait until
After being etched completely at the bottom of cuprio, the most remaining PMMA/ Graphene, fish for PMMA/ Graphene with the silicon chip of a diameter of 2cm, pick up sample
Product are put in clear water, wait about 5 minutes, then transfer in another part of clear water by same method, wait about 5min, then turn
Move on in the 3rd part of ready clean deionized water, wait about 5min；
(6) by target substrate (sheet glass or multi-layer film structure) by Graphene/PMMA picking up gently, blow by nitrogen gun
Dry (at this moment must note controlling air-flow, carefully dry up), in order to give a pressure the least, is got rid of
Water between PMMA/ Graphene and substrate；
(7) heat being placed on the drying glue platform of 150 DEG C by the sample of the PMMA/ Graphene/substrate flattened about
3min, finally takes out sample, is cooled to room temperature in atmosphere；
(8) acetone soak sample is used more than 15 hours, it is therefore an objective to remove the PMMA glue being attached with Graphene, then put by solution
50 DEG C of heating on drying glue platform, about about 3 hours, reach the effect removed photoresist further.
The femto-second laser that we used 400nm carrys out pumping perovskite, in order to get rid of mode competition and Mode Coupling
Impact.We have chosen the bar perovskite in the FP chamber only sending out single-mode laser, adjusts pump by the Glan prism in regulation light path
The size of Pu light energy, then record lead halide micron bar perovskite and be excited under different excitation energies the curve of spectrum of light,
By the process of fitting treatment of data, we obtain corresponding threshold curve, as shown in Fig. 3 (a).Then we are by micro-for same perovskite
On the Graphene that rice rod utilizes optical fiber to transfer to shift in advance by micromanipulative technique, record equally different pumping by force under
Laser spectrum, shown in fit threshold curve such as Fig. 3 (b).By the contrast of data, we can obtain clearly, and perovskite/
System and the Perovskite Phase of Graphene compare, and threshold value reduces nearly 20%, and the output light intensity under identical pump intensity increases
Nearly 4 times.
Above result, adds last layer two-dimensional material Graphene for we are simple exactly below perovskite, permissible
Effectively reduce the threshold value of perovskite, add the intensity of output light.So explaining its reason with regard to such phenomenon, we recognize
For, exactly because being in the following Graphene receptor as electronics or the suppression body of electronics, by perovskite/Graphene system
Electronics and the hole of interface efficiently separate, and reduce the binding energy between exciton, thus reduce the auger recombination of exciton.For
Checking Auger process, it is contemplated that to how effectively recording exciton under conditions of the perovskite of chemosynthesis can bear
Binding energy.Sample is put in liquid nitrogen cryogenics thermostat by we, by changing temperature scope from 10K to room temperature, surveys respectively
Amount perovskite and the fluorescence spectrum of perovskite/Graphene system, then the binding energy of exciton is gone out by Arrhenius equation model
(Eb).Result is as shown in Figure 4.By multiple authentication, we can obtain the exciton bind energy of perovskite is 14.8meV, and calcium
The exciton bind energy of titanium ore/Graphene system is 10.9meV, and it is sharp to perovskite that what this result will be apparent from indicates graphene layer
The impact of sub-binding energy, thus indirect verification Graphene can suppress the auger recombination of exciton.
Meanwhile, from the point of view of simple phenomenon, suppression therein is also embodied on the spectral width of laser spectrum, such as Fig. 5 institute
Show.We record perovskite and perovskite/graphene-structured respectively at 30uJ/cm2Low pumping density under fluorescence spectrum, logical
Crossing experiment to show, under identical pump intensity, the halfwidth of perovskite fluorescence spectrum is than the fluorescence spectrum of perovskite/Graphene
The little nearly 1nm of halfwidth.Therefore we may safely draw the conclusion, and when auger recombination is suppressed, the width of spectrum will increase.
Above content is to combine the further details of explanation that the present invention is done by concrete preferred implementation, but not
Represent the present invention be embodied as be limited to these explanations.For restraining the those of ordinary skill of neck belonging to the present invention,
Without departing from the inventive concept of the premise, it is also possible to make some simple deductions or replacement, be regarded as belonging to the present invention
Protection domain.
Claims (10)
1. the method utilizing two-dimensional material suppression perovskite auger recombination, it is characterised in that including: first chemical method is closed
Become perovskite micron order club shaped structure；Then shifted by wet method, shift Graphene on the glass substrate, add below perovskite
One layer of two-dimensional material Graphene, for the Raman spectrum of Graphene, the peak value at G peak and 2D peak is all higher than 0.8 × 10ka.u..
Method the most according to claim 1, it is characterised in that for the Raman spectrum of Graphene, the peak value at G peak is
The peak value at 8505a.u., 2D peak is 13845a.u..
Method the most according to claim 1 and 2, it is characterised in that described perovskite is CH3NH3PbBr3。
4. the system of perovskite/Graphene, it is characterised in that the system of described perovskite/Graphene passes through claim
Method described in 13 any claim prepares, and system and the Perovskite Phase of described perovskite/Graphene compare, threshold value
Reduce nearly 20%.
The system of perovskite/Graphene the most according to claim 4, it is characterised in that described perovskite/Graphene be
System and Perovskite Phase compare, and the output light intensity under identical pump intensity increases nearly 4 times.
The system of perovskite/Graphene the most according to claim 4, it is characterised in that described perovskite/Graphene be
System and Perovskite Phase compare, and exciton bind energy have dropped nearly 26%.
The system of perovskite/Graphene the most according to claim 4, it is characterised in that under identical pump intensity, calcium
The halfwidth nearly 1nm less than the halfwidth of the fluorescence spectrum of perovskite/Graphene of titanium ore fluorescence spectrum.
8. an electricity original paper, it is characterised in that containing the perovskite/Graphene described in claim 47 any claim
System.
A kind of electricity original paper the most according to claim 8, it is characterised in that described electricity refer to solaode,
The photovoltaic industry such as OLED.
A kind of electricity original paper the most according to claim 8, it is characterised in that described electricity original paper includes perovskite laser
Device, semiconductor laser etc..
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Cited By (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108793145A (en) * | 2018-06-30 | 2018-11-13 | 中国人民解放军国防科技大学 | Atomic-level-thickness graphene/boron nitride composite heterogeneous film and preparation |
| CN108793100A (en) * | 2018-06-30 | 2018-11-13 | 中国人民解放军国防科技大学 | Atomic-level thickness graphene/boron nitride composite heterogeneous film transfer method |
| CN111243971A (en) * | 2020-01-22 | 2020-06-05 | 华南理工大学 | Flexible substrate metal oxide thin film transistor and preparation method of passivation layer thereof |
Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103354273A (en) * | 2013-06-17 | 2013-10-16 | 华侨大学 | Embedded large-area flexible sensitized solar cell and preparation method thereof |
| CN104779352A (en) * | 2015-04-24 | 2015-07-15 | 苏州大学 | Light detector based on graphene and nano-structure perovskite material and manufacturing method |
| CN105671640A (en) * | 2015-12-29 | 2016-06-15 | 东南大学 | Layered large-size hybridized perovskite microcrystal material and preparation method thereof |
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2016
- 2016-07-08 CN CN201610536736.XA patent/CN106219600B/en not_active Expired - Fee Related
Patent Citations (3)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103354273A (en) * | 2013-06-17 | 2013-10-16 | 华侨大学 | Embedded large-area flexible sensitized solar cell and preparation method thereof |
| CN104779352A (en) * | 2015-04-24 | 2015-07-15 | 苏州大学 | Light detector based on graphene and nano-structure perovskite material and manufacturing method |
| CN105671640A (en) * | 2015-12-29 | 2016-06-15 | 东南大学 | Layered large-size hybridized perovskite microcrystal material and preparation method thereof |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN108793145A (en) * | 2018-06-30 | 2018-11-13 | 中国人民解放军国防科技大学 | Atomic-level-thickness graphene/boron nitride composite heterogeneous film and preparation |
| CN108793100A (en) * | 2018-06-30 | 2018-11-13 | 中国人民解放军国防科技大学 | Atomic-level thickness graphene/boron nitride composite heterogeneous film transfer method |
| CN111243971A (en) * | 2020-01-22 | 2020-06-05 | 华南理工大学 | Flexible substrate metal oxide thin film transistor and preparation method of passivation layer thereof |
| WO2021147284A1 (en) * | 2020-01-22 | 2021-07-29 | 华南理工大学 | Flexible substrate metal oxide thin film transistor and passivation layer preparation method thereof |
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